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The structural design of self-healing materials determines the ultimate performance of the product that can be used in a wide range of applications. Incorporating intrinsic self-healing moieties into puncture-resistant materials could significantly improve the failure resistance and product longevity, since their rapidly rebuilt bonds will provide additional recovery force to resist the external force. Herein, we present a series of tailored urea-modified poly(dimethylsiloxane)-based self-healing polymers (U-PDMS-SPs) that exhibit excellent puncture-resistant properties, fast autonomous self-healing, multi-cycle adhesion capabilities, and well-tunable mechanical properties. Controlling the composition of chemical and physical cross-links enables the U-PDMS-SPs to have an extensibility of 528% and a toughness of 0.6 MJ m −3 . U-PDMS-SPs exhibit fast autonomous self-healability with 25% strain recovery within 2 minutes of healing, and over 90% toughness recovery after 16 hours. We further demonstrate its puncture-resistant properties under the ASTM D5748 standard with an unbreakable feature. Furthermore, the multi-cycle adhesive properties of U-PDMS-SPs are also revealed. High puncture resistance (>327 mJ) and facile adhesion with rapid autonomous self-healability will have a broad impact on the design of adhesives, roofing materials, and many other functional materials with enhanced longevity. 

Abstract Metasurfaces, the ultra-thin media with extraordinary wavefront modulation ability, have shown great promise for many potential applications. However, most of the existing metasurfaces are limited by narrow-band and strong dispersive modulation, which complicates their real-world applications and, therefore require strict customized dispersion. To address this issue, we report a general methodology for generating ultra-broadband achromatic metasurfaces with prescribed ultra-broadband achromatic properties in a bottom-up inverse-design paradigm. We demonstrate three ultra-broadband functionalities, including acoustic beam deflection, focusing and levitation, with relative bandwidths of 93.3%, 120% and 118.9%, respectively. In addition, we reveal a relationship between broadband achromatic functionality and element dispersion. All metasurface elements have anisotropic and asymmetric geometries with multiple scatterers and local cavities that synthetically support internal resonances, bi-anisotropy and multiple scattering for ultra-broadband customized dispersion. Our study opens new horizons for ultra-broadband highly efficient achromatic functional devices, with promising extension to optical and elastic metamaterials.